Benchmarking Quantum Mechanical Levels of Theory for Valence Parametrization in Force Fields

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Abstract
A wide range of density functional methods and basis sets are available to derive the electronic structure and properties of molecules. Quantum mechanical calculations are too computationally intensive for routine simulation of molecules in the condensed phase, prompting the development of computationally efficient force fields based on quantum mechanical data. Parametrizing general force fields, which cover a vast chemical space, necessitates generating sizable quantum mechanical datasets with optimized geometries and torsion scans. To achieve this efficiently, it is crucial to choose a quantum mechanical method that balances computational cost and accuracy. In this study we seek to assess the accuracy of quantum mechanical theory for specific properties such as conformer energies, electrostatic properties, and torsion energetics. To comprehensively evaluate various methods, we focus on a representative set of 59 diverse small molecules, comparing approximately 24 combinations of functional and basis sets against the reference level coupled cluster calculations at complete basis set limit.
Funding Information
  • National Institute of Health Sciences (R01GM132386)
  • National Institute of Health Sciences (R35GM148236)
  • UK Research and Innovation (MR/T019654/1)
  • American Chemical Society Petroleum Research Fund (58158-DNI6)

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